Stabilization of low-valence transition metal towards advanced catalytic effects on the hydrogen storage performance of magnesium hydride
Magnesium hydride (MgH2) has been widely regarded as a potential hydrogen storage material owing to its high gravimetric and volumetric capacity. Its sluggish kinetics and high activation energy barrier, however, severely limit its practical application. Transition metal oxides (TMOs) have been exte...
Main Authors: | , , , , , , , |
---|---|
Format: | Article |
Language: | English |
Published: |
KeAi Communications Co., Ltd.
2021-03-01
|
Series: | Journal of Magnesium and Alloys |
Subjects: | |
Online Access: | http://www.sciencedirect.com/science/article/pii/S2213956720302085 |
id |
doaj-b83b6bf7f5da41e894a7cdc76481a943 |
---|---|
record_format |
Article |
spelling |
doaj-b83b6bf7f5da41e894a7cdc76481a9432021-04-18T06:27:21ZengKeAi Communications Co., Ltd.Journal of Magnesium and Alloys2213-95672021-03-0192647657Stabilization of low-valence transition metal towards advanced catalytic effects on the hydrogen storage performance of magnesium hydrideJian Zhang0Shuai Yan1Guanglin Xia2Xiaojie Zhou3Xianzheng Lu4Linping Yu5Xuebin Yu6Ping Peng7Hunan Provincial Key Laboratory of Intelligent Manufacturing Technology for High-performance Mechanical Equipment, Changsha University of Science and Technology, Changsha 410114, ChinaHunan Provincial Key Laboratory of Intelligent Manufacturing Technology for High-performance Mechanical Equipment, Changsha University of Science and Technology, Changsha 410114, ChinaDepartment of Materials Science, Fudan University, Shanghai 200433, China; Corresponding authors.Hunan Provincial Key Laboratory of Intelligent Manufacturing Technology for High-performance Mechanical Equipment, Changsha University of Science and Technology, Changsha 410114, ChinaHunan Provincial Key Laboratory of Intelligent Manufacturing Technology for High-performance Mechanical Equipment, Changsha University of Science and Technology, Changsha 410114, ChinaSchool of Chemistry and Biological Engineering, Changsha University of Science and Technology, Changsha 410114, ChinaDepartment of Materials Science, Fudan University, Shanghai 200433, China; Corresponding authors.College of Materials Science and Engineering, Hunan University, Changsha 410082, ChinaMagnesium hydride (MgH2) has been widely regarded as a potential hydrogen storage material owing to its high gravimetric and volumetric capacity. Its sluggish kinetics and high activation energy barrier, however, severely limit its practical application. Transition metal oxides (TMOs) have been extensively used as catalysts to improve the hydrogen storage performance of MgH2, but the low-valence transition metal (TM) ions, resulting from the reduction of TMOs accompanied by the formation of inactive MgO, have been demonstrated to be the most effective components. Herein, we theoretically and experimentally confirm that the doping of low-valence TMs into MgO could effectively weaken the Mg-H bonds and decrease the energy required for hydrogen desorption from MgH2, leading to superior catalytic activity compared to both TMOs and MgO. In particular, the apparent activation energy for the dehydrogenation of Mg(Nb)O-catalyzed MgH2 could be reduced to only 84.1 kJ mol-1, and the reversible capacity could reach around 7 wt.% after 5 cycles with a capacity retention of 96%. Detailed theoretical calculations confirm that the remarkable orbital hybridization between Mg(Nb)O and MgH2 promotes charge transfer from MgO to the MgH2 monomer, resulting in significantly weakened stability of MgH2, which could effectively enhance its hydrogen storage performance.http://www.sciencedirect.com/science/article/pii/S2213956720302085Magnesium hydrideHydrogen storageDehydrogenationCatalystsFirst-principles calculationsSolid-solution |
collection |
DOAJ |
language |
English |
format |
Article |
sources |
DOAJ |
author |
Jian Zhang Shuai Yan Guanglin Xia Xiaojie Zhou Xianzheng Lu Linping Yu Xuebin Yu Ping Peng |
spellingShingle |
Jian Zhang Shuai Yan Guanglin Xia Xiaojie Zhou Xianzheng Lu Linping Yu Xuebin Yu Ping Peng Stabilization of low-valence transition metal towards advanced catalytic effects on the hydrogen storage performance of magnesium hydride Journal of Magnesium and Alloys Magnesium hydride Hydrogen storage Dehydrogenation Catalysts First-principles calculations Solid-solution |
author_facet |
Jian Zhang Shuai Yan Guanglin Xia Xiaojie Zhou Xianzheng Lu Linping Yu Xuebin Yu Ping Peng |
author_sort |
Jian Zhang |
title |
Stabilization of low-valence transition metal towards advanced catalytic effects on the hydrogen storage performance of magnesium hydride |
title_short |
Stabilization of low-valence transition metal towards advanced catalytic effects on the hydrogen storage performance of magnesium hydride |
title_full |
Stabilization of low-valence transition metal towards advanced catalytic effects on the hydrogen storage performance of magnesium hydride |
title_fullStr |
Stabilization of low-valence transition metal towards advanced catalytic effects on the hydrogen storage performance of magnesium hydride |
title_full_unstemmed |
Stabilization of low-valence transition metal towards advanced catalytic effects on the hydrogen storage performance of magnesium hydride |
title_sort |
stabilization of low-valence transition metal towards advanced catalytic effects on the hydrogen storage performance of magnesium hydride |
publisher |
KeAi Communications Co., Ltd. |
series |
Journal of Magnesium and Alloys |
issn |
2213-9567 |
publishDate |
2021-03-01 |
description |
Magnesium hydride (MgH2) has been widely regarded as a potential hydrogen storage material owing to its high gravimetric and volumetric capacity. Its sluggish kinetics and high activation energy barrier, however, severely limit its practical application. Transition metal oxides (TMOs) have been extensively used as catalysts to improve the hydrogen storage performance of MgH2, but the low-valence transition metal (TM) ions, resulting from the reduction of TMOs accompanied by the formation of inactive MgO, have been demonstrated to be the most effective components. Herein, we theoretically and experimentally confirm that the doping of low-valence TMs into MgO could effectively weaken the Mg-H bonds and decrease the energy required for hydrogen desorption from MgH2, leading to superior catalytic activity compared to both TMOs and MgO. In particular, the apparent activation energy for the dehydrogenation of Mg(Nb)O-catalyzed MgH2 could be reduced to only 84.1 kJ mol-1, and the reversible capacity could reach around 7 wt.% after 5 cycles with a capacity retention of 96%. Detailed theoretical calculations confirm that the remarkable orbital hybridization between Mg(Nb)O and MgH2 promotes charge transfer from MgO to the MgH2 monomer, resulting in significantly weakened stability of MgH2, which could effectively enhance its hydrogen storage performance. |
topic |
Magnesium hydride Hydrogen storage Dehydrogenation Catalysts First-principles calculations Solid-solution |
url |
http://www.sciencedirect.com/science/article/pii/S2213956720302085 |
work_keys_str_mv |
AT jianzhang stabilizationoflowvalencetransitionmetaltowardsadvancedcatalyticeffectsonthehydrogenstorageperformanceofmagnesiumhydride AT shuaiyan stabilizationoflowvalencetransitionmetaltowardsadvancedcatalyticeffectsonthehydrogenstorageperformanceofmagnesiumhydride AT guanglinxia stabilizationoflowvalencetransitionmetaltowardsadvancedcatalyticeffectsonthehydrogenstorageperformanceofmagnesiumhydride AT xiaojiezhou stabilizationoflowvalencetransitionmetaltowardsadvancedcatalyticeffectsonthehydrogenstorageperformanceofmagnesiumhydride AT xianzhenglu stabilizationoflowvalencetransitionmetaltowardsadvancedcatalyticeffectsonthehydrogenstorageperformanceofmagnesiumhydride AT linpingyu stabilizationoflowvalencetransitionmetaltowardsadvancedcatalyticeffectsonthehydrogenstorageperformanceofmagnesiumhydride AT xuebinyu stabilizationoflowvalencetransitionmetaltowardsadvancedcatalyticeffectsonthehydrogenstorageperformanceofmagnesiumhydride AT pingpeng stabilizationoflowvalencetransitionmetaltowardsadvancedcatalyticeffectsonthehydrogenstorageperformanceofmagnesiumhydride |
_version_ |
1721523540689158144 |